Citation: Li Han, Li Fang, Yu Jiaguo, Cao Shaowen. 2D/2D FeNi-LDH/g-C₃N₄ Hybrid Photocatalyst for Enhanced CO₂ Photoreduction[J]. Acta Physico-Chimica Sinica, ;2021, 37(8): 201007. doi: 10.3866/PKU.WHXB202010073 shu

2D/2D FeNi-LDH/g-C₃N₄ Hybrid Photocatalyst for Enhanced CO₂ Photoreduction

State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China

Corresponding author: Cao Shaowen, swcao@whut.edu.cn
Received Date: 29 October 2020
Revised Date: 2 December 2020
Accepted Date: 2 December 2020
Available Online: 21 December 2020
Fund Project: the Natural Science Foundation of Hubei Province of China 2017CFA031the Fundamental Research Funds for the Central Universities, China 2020-YB-010the National Key Research and Development Program of China 2018YFB1502001the National Natural Science Foundation of China 51932007the Fundamental Research Funds for the Central Universities, China WUT: 2019-III-196the National Natural Science Foundation of China U1705251the National Natural Science Foundation of China 21773179the National Natural Science Foundation of China 51961135303the National Natural Science Foundation of China 51922081The authors acknowledge the financial support from the National Natural Science Foundation of China (51922081, 21773179, 51961135303, 51932007, U1705251) and the National Key Research and Development Program of China (2018YFB1502001), the Natural Science Foundation of Hubei Province of China (2017CFA031), and the Fundamental Research Funds for the Central Universities, China (WUT: 2019-III-196, 2020-YB-010)

Photocatalytic reduction of carbon dioxide into chemical fuels is a promising route to generate renewable energy and curtail the greenhouse effect. Therefore, various photocatalysts have been intensively studied for this purpose. Among them, g-C₃N₄, a 2D metal-free semiconductor, has been a promising photocatalyst because of its unique properties, such as high chemical stability, suitable electronic structure, and facile preparation. However, pristine g-C₃N₄ suffers from low solar energy conversion efficiency, owing to its small specific surface area and extensive charge recombination. Therefore, designing g-C₃N₄ (CN) nanosheets with a large specific surface area is an effective strategy for enhancing the CO₂ reduction performance. Unfortunately, the performance of CN nanosheets remains moderate due to the aforementioned charge recombination. To counter this issue, loading a cocatalyst (especially a two-dimensional (2D) one) can enable effective electron migration and suppress electron-hole recombination during photo-irradiation. Herein, CN nanosheets with a large specific surface area (97 m²·g^-1) were synthesized by a two-step calcination method, using urea as the precursor. Following this, a 2D/2D FeNi-LDH/g-C₃N₄ hybrid photocatalyst was obtained by loading a FeNi layered double hydroxide (FeNi-LDH) cocatalyst onto CN nanosheets by a simple hydrothermal method. It was found that the production rate of methanol from photocatalytic CO₂ reduction over the FeNi-LDH/g-C₃N₄ composite is significantly higher than that of pristine CN. Following a series of characterization and analysis, it was demonstrated that the FeNi-LDH/g-C₃N₄ composite photocatalyst exhibited enhanced photo-absorption, which was ascribed to the excellent light absorption ability of FeNi-LDH. The CO₂ adsorption capacity of the FeNi-LDH/g-C₃N₄ hybrid photocatalyst improved, owing to the large specific surface area and alkaline nature of FeNi-LDH. More importantly, the introduction of FeNi-LDH on the CN nanosheet surface led to the formation of a 2D/2D heterojunction with a large contact area at the interface, which could promote the interfacial separation of charge carriers and effectively inhibit the recombination of the photogenerated electrons and holes. This subsequently resulted in the enhancement of the CO₂ photo-reduction activity. In addition, by altering the loading amount of FeNi-LDH for photocatalytic performance evaluation, it was found that the optimal loading amount was 4% (w, mass fraction), with a methanol production rate of 1.64 μmol·h^-1·g^-1 (approximately 6 times that of pure CN). This study provides an effective strategy to improve the photocatalytic CO₂ reduction activity of g-C₃N₄ by employing 2D layered double hydroxide as the cocatalyst. It also proposes a protocol for the successful design of 2D/2D photocatalysts for solar energy conversion.
- Photocatalysis,
- 2D materials,
- Layered double hydroxide,
- Solar energy conversion,
- Charge transfer
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

2D/2D FeNi-LDH/g-C3N4 Hybrid Photocatalyst for Enhanced CO2 Photoreduction

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通讯作者: 陈斌, bchen63@163.com

2D/2D FeNi-LDH/g-C₃N₄ Hybrid Photocatalyst for Enhanced CO₂ Photoreduction